High-Pressure Fluidized Bed Reactor for Preparing Granular Polycrystalline Silicon

ABSTRACT

The present invention relates to a high-pressure fluidized bed reactor for preparing granular polycrystalline silicon, comprising (a) a reactor tube, (b) a reactor shell encompassing the reactor tube, (c) an inner zone formed within the reactor tube, where a silicon particle bed is formed and silicon deposition occurs, and an outer zone formed in between the reactor shell and the reactor tube, which is maintained under the inert gas atmosphere, and (d) a controlling means to keep the difference between pressures in the inner zone and the outer zone being maintained within the range of 0 to 1 bar, thereby enabling to maintain physical stability of the reactor tube and efficiently prepare granular polycrystalline silicon even at relatively high reaction pressure.

TECHNICAL FIELD

The present invention relates to a high-pressure fluidized bed reactorfor preparing granular polycrystalline silicon that enables to maintainlong-term stability of the reactor tube and efficiently prepare granularpolycrystalline silicon even at relatively high reaction pressure.

BACKGROUND ART

Generally, high-purity polycrystalline silicon is used as a basicmaterial for manufacturing semiconductor devices or solar cells. Thepolycrystalline silicon is prepared by thermal decomposition and/orhydrogen reduction of highly-purified silicon atom-containing reactiongas, thus causing the continuous silicon deposition on siliconparticles.

For mass production of polycrystalline silicon, a bell-jar type reactorhas been mainly used, which provides a rod-type polycrystalline siliconproduct with a diameter of about 50-300 mm. However, the bell-jar typereactor, which consists fundamentally of the electric resistance heatingsystem, cannot be operated continuously due to inevitable limit inextending the maximum rod diameter achievable. This reactor is alsoknown to have serious problems of low deposition efficiency and highelectrical energy consumption because of limited silicon surfaces andhigh heat loss.

Alternatively, a fluidized bed reactor has recently been developed toprepare granular polycrystalline silicon with a size of 0.5-3 mm.According to this method, a fluidized bed of silicon particles is formedby the upward flow of gas and the size of the silicon particlesincreases as the silicon atoms deposit on the particles from the siliconatom-containing reaction gas supplied to the heated fluidized bed.

As in the conventional bell-jar type reactor, the fluidized bed reactoralso uses a silane compound of Si—H—Cl system such as monosilane (SiH₄),dichlorosilane (SiH₂Cl₂), trichlorosilane (SiHCl₃), silicontetrachloride (SiCl₄) or its mixture as the silicon atom-containingreaction gas, which usually further comprises hydrogen, nitrogen, argon,helium, etc.

For the silicon deposition, the reaction temperature (i.e., temperatureof the silicon particles) should be maintained high. The temperatureshould be about 600-850° C. for monosilane, while being about 900-1,100°C. for trichlorosilane which is most widely used.

The process of silicon deposition, which is caused by thermaldecomposition and/or hydrogen reduction of silicon atom-containingreaction gas, includes various elementary reactions, and there arecomplex routes where silicon atoms grow into granular particlesdepending on the reaction gas. However, regardless of the kind of theelementary reaction and the reaction gas, the operation of the fluidizedbed reactor provides a granular polycrystalline silicon product.

Here, smaller silicon particles, i.e., seed crystals become bigger insize due to continuous silicon deposition or the agglomeration ofsilicon particles, thereby losing fluidity and ultimately movingdownwards. The seed crystals may be prepared or generated in situ in thefluidized bed itself, or supplied into the reactor continuously,periodically or intermittently. Thus prepared bigger particles, i.e.,polycrystalline silicon product may be withdrawn from the lower part ofthe reactor continuously, periodically or intermittently.

Due to the relatively high surface area of the silicon particles, thefluidized bed reactor system provides a higher reaction yield than thatby the bell-jar type reactor system. Further, the granular product maybe directly used without further processing for the following-upprocesses such as single crystal growth, crystal block production,surface treatment and modification, preparation of chemical material forreaction or separation, or molding or pulverization of siliconparticles. Although these follow-up processes have been operated in abatchwise manner, the manufacture of the granular polycrystallinesilicon allows the processes to be performed in a semi-continuous orcontinuous manner.

The increase in the productivity of the fluidized bed reactor isrequired for low-cost manufacture of granular polycrystalline silicon.For this purpose, it is most effective to increase the silicondeposition rate with low specific energy consumption, which isobtainable by continuous operation of the fluidized bed reactor underhigh pressure. For continuous operation of the process with thefluidized bed reactor, it is essential to secure the physical stabilityof the reactor components.

Unlike conventional fluidized bed reactors, serious limitations areencountered in material selection of the components of the fluidized bedreactor for preparing polycrystalline silicon. Especially, consideringthe desired high purity of the polycrystalline silicon, the materialselection of the fluidized bed wall is important. The reactor wall isweak in physical stability because it is always in contact with siliconparticles fluidizing at high temperatures, and is subject to theirregular vibration and severe shear stress caused by the fluidized bedof the particles. However, it is very difficult to select an appropriatematerial among the high-purity non-metallic inorganic materials that arecapable of enduring a relatively high pressure condition, becausemetallic material is not appropriate because of high reactiontemperature and chemical properties of the reaction gas. For thisreason, the fluidized bed reactor for manufacture of polycrystallinesilicon inevitably has a complicated structure. It is therefore commonthat a reactor tube made of quartz is positioned in an electricalresistance heater for heating the silicon particles, and both thereactor tube and the heater are surrounded by a metallic shell. It ispreferred to fill an insulating material in between the heater and thereactor shell or outside the reactor shell to reduce heat loss.

For example, U.S. Pat. No. 5,165,908 discloses a reactor system where anelectric resistance heater encloses a reactor tube made of quartz, bothof which are protected by a jacket-shaped stainless-steel shell and aninsulating material is installed outside the shell.

U.S. Pat. No. 5,810,934 discloses a fluidized bed reactor formanufacture of polycrystalline silicon, comprising a reactor vessel,i.e., the reactor tube defining a fluidized bed; a shroud, i.e., aprotection tube surrounding the reactor tube; a heater installed outsidethe shroud; and an outer containment surrounding the heater and aninsulating material. This patent emphasizes that the protection tubemade of quartz be installed in between the reactor tube and the heaterto prevent the crack of the reactor tube and the contamination of itsinner space.

Meanwhile, the fluidized bed reactor for manufacture of polycrystallinesilicon may have a different structure depending on the heating method.

For example, U.S. Pat. No. 4,786,477 discloses a method of heatingsilicon particles with microwave penetrating through the quartz reactortube instead of applying a conventional heater outside the tube.However, this patent still has a problem of a complex structure of thereactor and fails to disclose how to increase the reaction pressureinside the quartz reactor tube.

To solve the above problem, U.S. Pat. No. 5,382,412 discloses asimple-structured fluidized bed reactor for manufacture ofpolycrystalline silicon, wherein a cylindrical reactor tube is holdvertically by a metallic reactor shell. However, this patent still hasproblems that the inner pressure cannot be increased beyond atmosphericpressure and the microwave supplying means should be combined with thereactor shell, thus failing to suggest how to overcome the mechanicalweakness of the reactor tube that is anticipated at high-pressurereaction.

Therefore, in an embodiment of the present invention there is provided ahigh-pressure fluidized bed reactor for preparing granularpolycrystalline silicon, which comprises (a) a reactor tube, (b) areactor shell encompassing the reactor tube, (c) an inner zone formedwithin the reactor tube, where a silicon particle bed is formed andsilicon deposition occurs, and an outer zone formed in between thereactor shell and the reactor tube, which is maintained under an inertgas atmosphere, and (d) a controlling means to keep the differencebetween pressures in the inner zone and the outer zone being maintainedwithin the range of 0 to 1 bar, thereby enabling to maintain physicalstability of the reactor tube and efficiently prepare granularpolycrystalline silicon even at relatively high reaction pressure.

Further, in another embodiment of the present invention, there isprovided a fluidized bed reactor that can be conveniently applicable tothe manufacture of high-purity silicon particles while minimizing theimpurity contamination.

DISCLOSURE OF INVENTION

According to one aspect of the present invention, there is provided ahigh-pressure fluidized bed reactor for preparing granularpolycrystalline silicon, comprising:

-   -   (a) a reactor tube;    -   (b) a reactor shell encompassing the reactor tube;    -   (c) an inner zone formed within the reactor tube and an outer        zone formed in between the reactor shell and the reactor tube,        wherein a silicon particle bed is formed and silicon deposition        occurs in the inner zone while a silicon particle bed is not        formed and silicon deposition does not occur in the outer zone;    -   (d) an inlet means for introducing gases into the silicon        particle bed;    -   (e) an outlet means comprising a silicon particle outlet means        and a gas outlet means for discharging polycrystalline silicon        particles and off-gas out of the silicon particle bed,        respectively;    -   (f) an inert gas connecting means for maintaining a        substantially inert gas atmosphere in the outer zone;    -   (g) a pressure controlling means for measuring and/or        controlling the inner zone pressure (Pi) and the outer zone        pressure (Po); and    -   (h) a pressure-difference controlling means for maintaining        |Po−Pi| value in the range of 0-1 bar.

Referring to the Drawings herein, there is provided a detaileddescription of the present invention hereunder.

FIGS. 1 and 2 are cross-sectional views of the high-pressure fluidizedbed reactor for preparing granular polycrystalline silicon, in whichsome of the embodiments according to the present invention areillustrated in a comprehensive way.

An inner space of the fluidized bed reactor here is separated from anouter space by a reactor shell 1 that surrounds a vertically-installedreactor tube 2. The reactor tube 2 partitions the inner space into aninner zone 4, where a silicon particle bed is formed and silicondeposition occurs, and an outer zone 5, where a silicon particle bed isnot formed and silicon deposition does not occur.

The reactor shell 1 is preferred to be made of a metallic material withreliable mechanical strength and processability such as carbon steel,stainless steel or other alloy steel. The reactor shell 1 may be dividedinto a plurality of components such as 1 a, 1 b, 1 c and 1 d as setforth in FIGS. 1 and 2 for convenience in fabrication, assembly anddisassembly.

It is important to assemble the components of the reactor shell 1 byusing gaskets or sealing materials for complete sealing. The componentsmay have various structures of a cylindrical pipe, a flange, a tube withfittings, a plate, a cone, an ellipsoid and a double-wall jacket with acooling medium flowing in between the walls. The inner surface of eachcomponent may be coated with a protective layer or be installed with aprotective tube or wall, which may be made of a metallic material or anon-metallic material such as organic polymer, ceramic and quartz.

Some of the components of the reactor shell 1, illustrated as 1 a, 1 b,1 c and 1 d in FIGS. 1 and 2, are preferred to be maintained below acertain temperature by using a cooling medium such as water, oil, gasand air for protecting the equipment or operators, or for preventing anythermal expansion in equipment or a safety accident. Although not setforth in FIGS. 1 and 2, the components that need to be cooled arepreferred to be designed to comprise a coolant-circulating means attheir inner or outer walls. Instead of cooling, the reactor shell 1 maycomprise an insulating material on the outer wall.

The reactor tube 2 may be of any shape only if it can be hold by thereactor shell 1 in such a manner that it can separate the inner space ofthe reactor shell 1 into an inner zone 4 and an outer zone 5. Thereactor tube 2 may be of a structure of a simple straight tube as inFIG. 1, a shaped tube as in FIG. 2, a cone or an ellipsoid, and eitherone end or both ends of the reactor tube 2 may be formed into a flangeshape. Further, the reactor tube 2 may comprise a plurality ofcomponents and some of these components may be installed in the form ofa liner on the inner wall of the reactor shell 1.

The reactor tube 2 is preferred to be made of an inorganic material,which is stable at a relatively high temperature, such as quartz,silica, silicon nitride, boron nitride, silicon carbide, graphite,silicon, glassy carbon or their combination.

Meanwhile, a carbon-containing material such as silicon carbide,graphite, glassy carbon may generate carbon impurity and contaminate thepolycrystalline silicon particles. Thus, if the reactor tube 2 is madeof a carbon-containing material, the inner wall of the reactor tube 2 ispreferred to be coated or lined with materials such as silicon, silica,quartz or silicon nitride. Then, the reactor tube 2 may be structured ina multi-layered form. Therefore, the reactor tube 2 is of one-layered ormultilayered structure in the thickness direction, each layer of whichis made of a different material.

Sealing means 41 a, 41 b may be used for the reactor shell 1 to safelyhold the reactor tube 2. The sealing means are preferred to be stable ata temperature of above 200° C. and may be selected from organic polymer,graphite, silica, ceramic, metal or their combination. However,considering the vibration and thermal expansion during reactoroperation, the sealing means 41 a, 41 b may be installed less firmly tolower the possibility of cracking of the reactor tube 2 in the course ofassembly, operation and disassembly.

The partition of the inner space of the reactor shell 1 by the reactortube 2 may prevent the silicon particles in the inner zone 4 fromleaking into the outer zone 5 and differentiate the function andcondition between the inner zone 4 and the outer zone 5.

In the meantime, a heating means 8 a, 8 b may be installed in thereactor shell 1 to heat silicon particles. One or a plurality of heatingmeans 8 a, 8 b may be installed in the inner zone 4 and/or the outerzone 5 in various manner. For example, a heating means may be installedonly in the inner zone 4 or in the outer zone 5 as illustrated in FIG. 1in a comprehensive manner. Meanwhile, a plurality of heating means maybe installed in both zones, or only in the outer zone 5 as illustratedin FIG. 2. Besides, although it is not illustrated in Drawings, aplurality of heating means 8 a, 8 b may be installed only in the innerzone 4. Otherwise, a single heating means may be installed in the outerzone 5 only.

The electric energy is supplied to the heating means 8 a, 8 b through anelectric energy supplying means 9 a-9 f installed on or through thereactor shell 1. The electric energy supplying means 9 a-9 f, whichconnects the heating means 8 a, 8 b in the reactor and an electricsource E outside the reactor, may comprise a metallic component in theform of a cable, a bar, a rod, a shaped body, a socket or a coupler.Otherwise the electric energy supplying means 9 a-9 f may comprise anelectrode that is made of a material such as graphite, ceramic (e.g.,silicon carbide), metal or a mixture thereof, and is fabricated invarious shapes. Alternatively, the electric energy supplying means canbe prepared by extending a part of the heating means 8 a, 8 b. Incombining the electric energy supplying means 9 a-9 f with the reactorshell 1, electrical insulation is also important besides the mechanicalsealing for preventing gas leak. Further, it is desirable to cool downthe temperature of the electric energy supplying means 9 by using acirculating cooling medium such as water, oil and gas.

Meanwhile, a gas inlet means should be installed at the fluidized bedreactor to form a fluidized bed, where silicon particles can move by gasflow, within the reactor tube 2, i.e., in a lower part of the inner zone4, for preparation of polycrystalline silicon by the silicon depositionon the surface of the fluidizing silicon particles.

The gas inlet means comprises a fluidizing gas inlet means 14, 14′ forintroducing a fluidizing gas 10 into the silicon particles bed and areaction gas inlet means 15 for introducing a silicon atom-containingreaction gas, both of which are installed in combination with thereactor shell 1 b.

As used herein, “a fluidizing gas” 10 refers to a gas introduced tocause some or most of the silicon particles 3 to be fluidized in thefluidized bed formed within the inner zone 4. In the present invention,hydrogen, nitrogen, argon, helium, hydrogen chloride (HCl), silicontetrachloride (SiCl4) or a mixture thereof may be used as the fluidizinggas 10.

As used herein, “a reaction gas” 11 refers to a source gas containingsilicon atoms, which is used to prepare the polycrystalline siliconparticles. In the present invention, monosilane (SiH4), dichlorosilane(SiH2Cl2), trichlorosilane (SiHCl3), silicon tetrachloride (SiCl4) or amixture thereof may be used as the reaction gas 11. The reaction gas 11may further comprise at least one gas selected from hydrogen, nitrogen,argon, helium and hydrogen chloride (HCl). Further, in addition toserving as a source for silicon deposition, the reaction gas 11contributes to the fluidization of the silicon particles 3 as thefluidizing gas 10 does.

The fluidizing gas inlet means 14, 14′ and the reaction gas inlet means15 may comprise a tube or nozzle, a chamber, a flange, a fitting, agasket, etc, respectively. Among these components, the parts exposed tothe inner space of the reactor shell 1, especially to the lower part ofthe inner zone 4, where the parts are likely to contact the siliconparticles 3, are preferred to be made of a tube, a liner or a shapedarticle the material of which is selected from those applicable to thereactor tube 2.

Further, the lower part of the fluidized bed 4 a in the inner zone 4 maycomprise a gas distributing means 19 for distributing the fluidizing gas10 in combination with the fluidizing gas inlet means 14, 14′ and thereaction gas inlet means 15. The gas distributing means 19 may have anygeometry or structure including a multi-hole or porous distributionplate, a packing filler material submerged in the particle bed, a nozzleor a combination thereof.

To prevent silicon deposition on the upper surface of the gasdistributing means 19, the outlet of the reaction gas inlet means 15,through which a reaction gas 11 is injected into the interior of thefluidized bed, is preferred to be positioned higher than the upper partof the gas distributing means 19.

In the reactor inner zone 4, the fluidizing gas 10, which is required toform the fluidized bed 4 a of silicon particles, may be supplied invarious ways depending on how the fluidizing gas inlet means 14, 14′ isconstituted. For example, as illustrated in FIG. 1, the fluidizing gas10 may be supplied by a fluidizing gas inlet means 14, 14′ coupled withthe reactor shell 1 so that a gas chamber may be formed in lower part ofthe distribution plate-shaped gas distributing means 19. Alternatively,as illustrated in FIG. 2, a fluidizing gas 10 may be supplied by afluidizing gas inlet means 14 coupled with the reactor shell 1 so thatone or a plurality of fluidizing gas nozzle outlet may be positioned inbetween the gas distributing means 19 that comprises a third packingfiller material other than those fluidizing silicon particles.Meanwhile, the gas distributing means 19 and the fluidizing gas inletmeans 14, 14′ may be constituted by using both the distribution plateand the packing filler material.

In the present invention, the polycrystalline silicon particles areprepared in the inner zone 4 of the reactor based on the silicondeposition. Following the supply of the reaction gas 11 through thereaction gas inlet means 15, the silicon deposition occurs on thesurface of the silicon particles 3 heated by the heating means 8 a, 8 b.

A particle outlet means 16 is also required to be combined with thereactor shell 1 to discharge thus prepared silicon particles from theinner zone 4 to the outside of the fluidized bed reactor.

An outlet pipe, which constitutes the particle outlet means 16, may beassembled with the reaction gas inlet means 15 as illustrated in FIG. 1.Alternatively, it may be installed independently of the reaction gasinlet means 15 as illustrated in FIG. 2. Through the particle outletmeans 16 the silicon particles 3 b may be discharged when required fromthe fluidized bed 4 a in a continuous, periodic, or intermittent way.

As illustrated in FIG. 1, an additional zone may be combined with thereactor shell 1. The additional zone can be provided at some part or alower part of the fluidizing gas inlet means 14′, allowing a space forthe silicon particles 3 b to reside or stay with an opportunity ofcooling before being discharged from the reactor.

Silicon particles 3, i.e., silicon particles 3 discharged from the innerzone 4 according to the present invention, may be delivered to a storagemember or a transfer member of the polycrystalline silicon product,which is directly connected to the reactor. Meanwhile, thus-preparedsilicon product particles 3 b may have a particle-size distribution dueto nature of the fluidized bed reactor, and smaller particles includedtherein may be used as seed crystals 3 a for the silicon deposition. Itis thus possible that the silicon product particles 3 b discharged fromthe inner zone 4 may be delivered to a particle separation member wherethe particles can be separated by size. Then the larger particles may bedelivered to the storage member or the transfer member, while thesmaller particles are used as seed crystals 3 a.

Otherwise, considering the relatively high-temperature of the siliconparticle fluidized bed 4 a, the silicon particles 3 b are preferred tobe cooled down while being discharged through the particle outlet means16. For this purpose, a cooling gas such as hydrogen, nitrogen, argon,helium, or a mixture thereof may flow in the particle outlet means 16,or a cooling medium such as water, oil or gas may be circulated throughthe wall of the particle outlet means 16.

Alternatively, although it is not illustrated in Drawings, the particleoutlet means 16 may be constituted in combination with the inner spaceof the reactor shell 1 (e.g. 14′ in FIG. 1) or a lower part of thereactor shell (e.g., 1 b in FIGS. 1 and 2), allowing a sufficient spacefor the silicon particles 3 b to reside or stay with an opportunity ofcooling for a certain period of time before being discharged from thereactor.

It is necessary to prevent the silicon product particles 3 b from beingcontaminated while discharged from the reactor through the particleoutlet means 16. Therefore, in constituting the particle outlet means16, the elements that may contact high-temperature silicon productparticles 3 b may be made of a tube, a liner or a shaped product that ismade of or coated with an inorganic material applicable to the reactortube 2. These elements of the particle outlet means 16 are preferred tobe coupled to the metallic reactor shell and/or a protection pipe.

The components of the particle outlet means 16, which are in contactwith the relatively low-temperature product particles or comprise acooling means on their wall, may be made of a metal-material tube, aliner or a shaped product, the inner wall of which is coated or linedwith a fluorine-containing polymer material.

As mentioned above, the silicon product particles 3 b may be dischargedfrom the reactor inner zone 4 through the particle outlet means 16 to astorage member or a transfer member of the polycrystalline siliconproduct in a continuous, periodic, or intermittent way.

Meanwhile, a particle separation member may be installed in between thereactor and the product storage member, to separate the silicon productparticles 3 b by size and use small-sized particles as seed crystals 3a. Various commercial devices may be used as the particle separationmember in the present invention.

It is desirable to constitute the elements of the particle separationmember, which may be in contact with the silicon product particles 3 b,by using the same material as the one used in the particle outlet means16, or pure polymer material that does not contain either an additive ora filler.

For continuous operation of the fluidized bed reactor, it is necessaryto combine the reactor shell 1 d with a gas outlet means 17 which isinstalled for discharging the off-gas from the fluidized bed reactor.The off-gas 13 comprises a fluidizing gas, a non-reacted reaction gasand a product gas, and passes through the upper part of the inner zone,4 c.

Fine silicon particles or high-molecular-weight byproducts entrained inthe off-gas 13 may be separated from an additional off-gas treatingmeans 34.

As illustrated in FIGS. 1 and 2, an off-gas treating means 34, whichcomprises a cyclone, a filter, a packed column, a scrubber or acentrifuge, may be installed outside the reactor shell 1 or at the upperzone 4 c of the inner zone within the reactor shell 1.

Fine silicon particles, thus separated from the off-gas treating means34, may be used for another purpose, or as seed crystals 3 a forpreparing silicon particles after being recycled into the fluidized bed4 a at the inner zone of the reactor.

When manufacturing silicon particles in a continuous manner, it ispreferred to maintain the number and the average particle size of thesilicon particles, which forms the fluidized bed 4 a, within a certainrange. This may be obtained by supplementing nearly the same number ofthe seed crystals within the fluidized bed 4 a as that of the dischargedsilicon product particles 3 b.

As mentioned above, the fine silicon particles or powders separated fromthe off-gas treating means 34 may be recycled as seed crystals, buttheir amount can not be sufficient. It is then required to furtheryield, generate or prepare additional silicon seed crystals forcontinuous preparation of the silicon particles as required in thefluidized bed.

In this regard, it may be considered to further separate the smallersilicon particles among the silicon product particles 3 b and use themas seed crystals 3 a. However, the additional process for separatingseed crystals 3 a from the product particles 3 b outside the fluidizedbed reactor has drawbacks of high chances of contamination anddifficulties in operation.

Instead of the additional separation of product particles 3 b, it isalso obtainable to cool silicon product particles 3 b, to separatesmaller particles out of them and to recycle the smaller particles asseed crystals into the fluidized bed. To this purpose an additionalparticle separation member may be installed in the middle of a dischargepath included in the particle outlet means 16. Supplying a gas into thepathway in a counter-current manner leads to cooling of the productparticles 3 b, separation of smaller particles out of them and recyclingof the smaller particles into the fluidized bed 4 a. This reduces theburden of preparing or supplying seed crystals, and increases theaverage particle size of the final silicon product particles 3 b whiledecreasing their particle size distribution.

As another embodiment, the silicon seed crystals may be prepared bypulverizing some of silicon product particles 3 b discharged through theparticle outlet means 16 into seed crystals in a separate pulverizingapparatus. Thus prepared seed crystals 3 a may be introduced into theinner zone 4 of the reactor in a continuos, periodic or intermittentlyway as required. One example when seed crystals 3 a is downwardlyintroduced into the inner zone 4 is illustrated in FIG. 1, where a seedcrystals inlet means 18 is combined with the topside of the reactorshell 1 d. This method allows an efficient control in the average sizeand the feeding rate of seed crystals 3 a as required, while it has adrawback of requiring a separate pulverizing apparatus.

On the contrary, silicon particles may be pulverized into seed crystalsinside fluidized bed 4 a by using an outlet nozzle of a reaction gasinlet means 15 combined with the reactor shell or an additionallyinstalled gas nozzle for a high-speed gas jet inside the fluidized bedallowing particle pulverization. This method has an economic advantagebecause it needs no additional pulverizing device, while having adrawback that it is difficult to control the size and generation amountof the seed crystals in the reactor within a predetermined acceptablerange.

In the present invention, the inner zone 4 comprises all spaces requiredfor forming a silicon particle bed 4 a, supplying a fluidizing gas 10and a reaction gas 11 into the silicon particle bed 4 a, allowingsilicon deposition, and discharging the off-gas 13 containing afluidizing gas, a non-reacted reaction gas and a byproduct gas.Therefore, the inner zone 4 plays a fundamental role for silicondeposition in the fluidized bed of silicon particles 3 and preparationof polycrystalline silicon product particles.

In contrast to the inner zone 4, the outer zone 5 is an independentlyformed space in between outer wall of reactor tube 2 and reactor shell1, where a silicon particle bed 3 is not formed and silicon depositiondoes not occur due to no supply of the reaction gas.

According to the present invention, the outer zone 5 also playsimportant roles as follows. First, the outer zone 5 provides a space forprotecting the reactor tube 2 by maintaining pressure difference betweenthe inner zone 4 and the outer zone 5 within a certain range.

Second, the outer zone 5 provides a space for installing an insulatingmaterial 6 that prevents or decreases heat loss from the reactor.

Third, the outer zone 5 provides a space for a heater to be installedaround the reactor tube 2.

Fourth, the outer zone 5 provides a space for maintaining asubstantially inert gas atmosphere outside the reactor tube 2 to preventdangerous gas containing oxygen and impurities from being introducedinto the inner zone 4, and for safely installing and maintaining thereactor tube 2 inside the reactor shell 1.

Fifth, the outer zone 5 allows a real-time monitoring of the status ofthe reactor tube 2 during operation. The analysis or measurement of theouter-zone gas sample from the outer zone connecting means 28 may revealthe presence or concentration of a gas component that may exist in theinner zone 4, the change of which may indirectly reveal an accident atthe reactor tube.

Sixth, the outer zone 5 provides a space for installing a heater 8 bsurrounding the reactor tube 2, as illustrated in FIG. 2, for heating upand chemically removing the silicon deposit layer accumulated on theinner wall of the reactor tube 2 due to silicon deposition operation.

Seventh, the outer zone 5 provides a space required for efficientlyassemblying or disassemblying the reactor tube 2 and the inner zone 4.

According to the present invention, the outer zone 5 plays variousimportant roles as mentioned above. Thus, the outer zone may bepartitioned into several sections in an up-and-down and/or a radial orcircumferential direction, utilizing one or more of tubes, plates,shaped articles or fittings as partitioning means.

When the outer zone 5 is further partitioned according to the presentinvention, the divided sections are preferred to be spatiallycommunicated with each other while having substantially the sameatmospheric condition and pressure.

An insulating material 6, which may be installed in the outer zone 5 forgreatly reducing heat transfer via radiation or conduction, may beselected from industrially acceptable inorganic materials in the form ofa cylinder, a block, fabric, a blanket, a felt, a foamed product, or apacking filler material.

The heating means 8 a, 8 b, connected to an electric energy supplyingmeans 9, which is connected to the reactor shell for maintainingreaction temperature in the fluidized bed reactor, may be installed inthe outer zone 5 only, or installed alone within the inner zone 4,especially within the silicon particle bed 4 a. The heating means 8 a, 8b, may be installed in both the inner zone 4 and the outer zone 5, ifrequired, as illustrated in FIG. 1. FIG. 2 illustrates an example when aplurality of independent heating means 8 a, 8 b are installed in theouter zone 5.

When a plurality of heating means 8 a, 8 b are installed in thefluidized bed reactor, they may be electrically connected in series orparallel relative to an electric source E. Alternatively, the powersupplying system comprising an electric source E and an electric energysupplying means 9 a-9 f may be constituted independently as illustratedin FIGS. 1 and 2.

As illustrated in FIG. 1, the heater 8 a installed within the siliconparticle bed 4 a may have an advantage of directly heating siliconparticles in the fluidized bed. In this case, to prevent accumulativesilicon deposition on the surface of the heater 8 a, the heater 8 a ispreferred to be positioned lower than the reaction gas outlet of areaction gas inlet means 15.

In the present invention, an inert gas connecting means 26 a, 26 b isinstalled on the reactor shell, independently of the inner zone 4, tomaintain a substantially inert gas atmosphere in the outer zone 5precluding silicon deposition. The inert gas 12 may be one or moreselected from hydrogen, nitrogen, argon and helium.

An inert gas connecting means 26 a, 26 b, which is installed on orthrough the reactor shell and spatially connected to the outer zone 5,has the function of piping connection for supplying or discharging aninert gas 12, and may be selected from a tube, a nozzle, a flange, avalve, a fitting or their combination.

Meanwhile, apart from the inert gas connecting means 26 a, 26 b, areactor shell, which is spatially exposed to the outer zone 5 directlyor indirectly, may be equipped with an outer zone connecting means 28.Then, the outer zone connecting means 28 may be used to measure andcontrol temperature, pressure or gas component. Although even a singleinert gas connecting means 26 a, 26 b may allow to maintain asubstantially inert gas atmosphere in the outer zone 5, the supply ordischarge of an inert gas may be independently performed by using adouble-pipe or a plurality of inert gas connecting means 26 a, 26 b.

Further, the inert gas connecting means 26 a, 26 b maintains anindependent inert gas atmosphere in the outer zone 5, and may also beused for measuring and/or controlling flow rate, temperature, pressureor gas component, which can also be performed by using the outer zoneconnecting means 28.

FIGS. 1 and 2 provide various examples in a comprehensive way wherepressure (Po) in the outer zone 5 is measured or controlled by using theinert gas connecting means 26 a, 26 b or outer zone connecting means 28.

The outer zone connecting means 28 may be installed to measure and/orcontrol the maintenance of the outer zone 5, independently of or onbehalf of the inert gas connecting means 26 a, 26 b. The outer zoneconnecting means 28 has the function of piping connection, and may beselected from a tube, a nozzle, a flange, a valve, a fitting or theircombination. If the inert gas connecting means 26 a, 26 b is notinstalled, the outer zone connecting means 28 may be used to supply ordischarge an inert gas 12 as well as to measure or control temperature,pressure or gas component. Therefore, it is not necessary todifferentiate the inert gas connecting means 26 a, 26 b from the outerzone connecting means 28 in respect of shape and function.

Unlike the outer zone 5, where pressure may be maintained nearlyconstant irrespective of position and time, there exists inevitably apressure difference within the inner zone 4 according to the height ofthe fluidized bed 4 a of silicon particles 3. Thus, pressure (Pi) in theinner zone 4 changes according to the height in the inner zone 4.

Although the pressure drop imposed by the fluidized bed of solidparticles depends on the height of the fluidized bed, it is common tomaintain the pressure drop by fluidized bed less than about 0.5-1 barunless the height of the fluidized bed is excessively high. Further,irregular fluctuation of the pressure is inevitable with time due to thenature of the fluidization of solid particles. Thus, pressure may varyin the inner zone 4 depending on position and time.

Considering these natures, the pressure controlling means for the innerpressure, i.e., the inner pressure controlling means 30 for directly orindirectly measuring or controlling pressure (Pi) in the inner zone 4may be installed at such a point among various positions that it may bespatially connected to the inner zone 4.

Pressure controlling means according to the present invention, i.e., theinner pressure controlling means 30 and the outer pressure controllingmeans 31 may be installed on or through various positions depending onthe details of the reactor assembly as well as on the operationalparameters to be controlled.

The pressure controlling means for the inner pressure, i.e., the innerpressure controlling means 30 may be spatially connected to the innerzone 4 through an inner zone connecting means 24, 25, a fluidizing gasinlet means 14, a reaction gas inlet means 15, a particle outlet means16, or a gas outlet means 17, which are spatially exposed directly orindirectly to the inner zone 4.

Meanwhile, the pressure controlling means for the outer pressure, i.e.,the outer pressure controlling means 31 may be spatially connected tothe outer zone 5 through an outer zone connecting means 28 or an inertgas connecting means 26 a, 26 b, etc., which are installed on or throughthe reactor shell 1 and spatially exposed directly or indirectly to theouter zone 5.

According to a preferable embodiment of the present invention, the innerpressure controlling means 30 and outer pressure controlling means 31comprise the components necessary for directly or indirectly measuringand/or controlling pressure.

Either of the pressure controlling means, 30 and 31, comprises at leastone selected from the group consisting of: (a) a connecting pipe orfitting for spatial connection; (b) a manually-operated, semi-automatic,or automatic valve; (c) a digital- or analog-type pressure gauge orpressure-difference gauge; (d) a pressure indicator or recorder; and (e)an element constituting a controller with a signal converter or anarithmetic processor.

The pressure controlling means for the inner pressure, 30, isinterconnected with the pressure controlling means for the outerpressure, 31, in the form of a mechanical assembly or a signal circuit.Further, either of the pressure controlling means may be partially orcompletely integrated with a control system selected from the groupconsisting of a central control system, a distributed control system anda local control system.

Although the inner pressure controlling means 30 and outer pressurecontrolling means 31 may be independently constituted in terms ofpressure, either of the pressure controlling means may be partially orcompletely integrated with a means for measuring or controlling aparameter selected from the group consisting of flow rate, temperature,gas component and particle concentration, and etc.

Meanwhile, either of the controlling means, 30 or 31, may furthercomprise a separation device such as a filter or a scrubber forseparating particles, or a container for buffering pressure. Thisprotects the component of the pressure controlling means fromcontamination by impurities, and also provides a means to bufferpressure changes.

As an example, the inner pressure controlling means 30 may be installedat or connected to the inner zone connecting means 24, 25, which isinstalled on or through the reactor shell and is spatially exposeddirectly or indirectly to an inner zone 4 for measurement of pressure,temperature or gas component or for viewing inside the reactor. Byconstructing the inner pressure controlling means 30 so that it may beconnected to the inner zone connecting means 24, 25, pressure in upperpart of the inner zone 4 c may be stably measured and/or controlledalthough it is difficult to detect the time-dependent pressurefluctuation due to the fluidized bed of silicon particles. For moreaccurate detection of the time-dependent pressure fluctuation relatedwith the fluidized bed, the inner zone connecting means may be installedso that it may be spatially connected to the inside of the fluidizedbed. The inner pressure controlling means 30 may also be installed at orconnected to other appropriate positions, i.e., a fluidizing gas inletmeans 14 or a reaction gas inlet means 15 or a particle outlet means 16or a gas outlet means 17, etc., all of which are combined with thereactor shell thus being spatially connected to the inner zone 4.

Further, a plurality of inner pressure controlling means 30 may beinstalled at two or more appropriate positions which ultimately allowspatial connection with the inner zone 4 through the inner zoneconnecting means 24, 25 or those at other positions (14, 15, 16, 17).

As mentioned above, the presence of silicon particles affects the innerpressure, Pi. Thus, the measured value of Pi varies according to theposition where the inner pressure controlling means 30 is installed.Following observations by the present inventors, the value of Pi isinfluenced by the characteristics of the fluidized bed and by thestructure of a fluidizing gas inlet means 14 or a reaction gas inletmeans 15 or a particle outlet means 16 or a gas outlet means 17, but itspositional deviation according to pressure measurement point is notgreater than 1 bar.

As a preferred embodiment, the outer pressure controlling means 31, fordirectly or indirectly measuring and/or controlling pressure in theouter zone 5, is preferred to be installed so that it may be spatiallyconnected to the outer zone 5. The position where the outer pressurecontrolling means 31 may be connected or installed includes, forexample, an outer zone connecting means 28 or an inert gas connectingmeans 26 a, 26 b installed on or through the reactor shell, which isspatially connected to the outer zone 5 directly or indirectly. In thepresent invention, the outer zone 5 is preferred to be maintained undera substantially inert gas atmosphere. Thus, the outer zone connectingmeans 28 may also comprise the function of an inert gas connecting means26 a that may be used for introducing an inert gas 12 to the outer zone5 or an inert gas connecting means 26 b that may be used for dischargingan inert gas 12 from the outer zone 5. Therefore, it is possible tospatially connect the outer zone 5 to the outer pressure controllingmeans 31 for directly or indirectly measuring and/or controllingpressure in the outer zone 5 through an inert gas connecting means 26 a,26 b or an outer zone connecting means 28.

In the present invention, the inner pressure controlling means 30 andthe outer pressure controlling means 31 may be used to maintain thevalue of |Po−Pi|, i.e. the difference between the pressure in the innerzone 4 (Pi) and that in the outer zone 5 (Po) within 1 bar. However, itshould be noted in constituting the inner pressure controlling means 30that Pi may vary depending on the position selected for connection tothe inner zone.

The value of Pi measured through an inner zone connecting means 24, 25,a fluidizing gas inlet means 14, a reaction gas inlet means 15, or aparticle outlet means 16, etc., which are installed at the positionsspatially connected to an inner or lower part of the fluidized bed, ishigher than the value of Pi measured through an inner zone connectingmeans, a gas outlet means 17 or silicon seed crystals inlet means 18,etc., which are installed at the positions spatially connected to aspace like an upper part of the inner zone 4 c and are not in directcontact with the fluidized bed of silicon particles.

Especially, the pressure value, measured through an inner zoneconnecting means, a fluidizing gas inlet means 14 or a particle outletmeans 16, which is spatially connected to a lower part of the fluidizedbed of silicon particles, shows a maximum inner pressure value,Pi_(max). On the contrary, a minimum inner pressure value, Pi_(min), maybe obtained when measured through a gas outlet means 17 or an inner zoneconnecting means 24, 25, which is not in direct contact with thefluidized bed. This is because there is a pressure difference dependingon the height of the fluidized bed of silicon particles 4 a and thevalue of Pi is always higher in the lower part as compared to the upperpart of the fluidized bed.

This pressure difference increases with the height of the fluidized bed.An excessively high bed with the pressure difference being 1 bar orhigher is not preferred because the height of the reactor becomes toohigh to be used. In contrast, a very shallow bed with the pressuredifference of 0.01 bar or lower is not preferred either, because theheight and volume of the fluidized bed is too small to achieve anacceptable minimum productivity of the reactor.

Therefore, the pressure difference in the fluidized bed is preferred tobe within the range of 0.01-1 bar. That is, pressure differences betweenmaximum pressure value (Pi_(max)) and minimum pressure value (Pi_(min))in the inner zone 4 is preferred to be within 1 bar.

When maintaining the value of |Po−Pi|, i.e. pressure difference betweeninside and outside the reactor tube 2 within the range of 0 to 1 bar, itshould be noted that the pressure difference may vary depending on theheight of the reactor tube 2.

It is preferred to meet the requirements of Po≦Pi and 0 bar≦(Pi−Po)≦1bar, when the inner pressure controlling means 30 is spatially connectedto the inner zone 4 through an inner zone connecting means, a fluidizinggas inlet means 14, a reaction gas inlet means 15 or a particle outletmeans 16, etc., which is connected to an inner or lower part of thefluidized bed of silicon particles, the pressure of which is higher thanthat of the upper part of the inner zone 4 c.

In contrast, it is preferred to meet the requirements of Pi≦Po and 0bar≦(Po−Pi)≦1 bar, when the inner pressure controlling means 30 isspatially connected to the inner zone 4 through a gas outlet means 17, asilicon seed crystals inlet means 18, or an inner zone connecting means24, 25, etc., which is not spatially connected to the fluidized bed ofsilicon particles but connected to an upper part of the inner zone 4 c,the pressure of which is lower than that of the inner or lower part ofthe fluidized bed.

It may also be permissible to constitute the inner pressure controllingmeans 30 or the outer pressure controlling means 31 in such manner thatPi or Po is represented by an average of a plurality of pressure valuesmeasured at one or more positions. Especially, because there may bepressure difference in the inner zone 4 depending on the connectionposition, the inner pressure controlling means 30 may comprise acontrolling means with an arithmetic processor that is capable ofestimating an average value of pressure from those values measured withtwo or more pressure gauges.

Therefore, when maintaining the value of |Po−Pi|, i.e., the pressuredifference value between inside and outside the reaction tube, within 1bar, it is preferred to maintain the pressure value at outer zone 5, Po,in between Pi_(max) and Pi_(min), which are maximum and minimum values,respectively, that can be measured by the spatial connection of thosepressure controlling means to the inner zone 4.

The inner pressure controlling means 30 and/or outer pressurecontrolling means 31 according to the present invention should comprisea pressure-difference controlling means that maintains the value of|Po−Pi| within 1 bar.

The pressure-difference controlling means may be comprised in only oneof the inner pressure controlling means 30 or the outer pressurecontrolling means 31, or in both of the controlling means independently,or in the two controlling means 30, 31 in common.

However, it is preferred to apply and maintain a pressure-differencecontrolling means with consideration that pressure value variesdepending on the position selected for measuring the pressure at theinner zone 4, Pi. When Pi is measured through a fluidizing gas inletmeans 14, a reaction gas inlet means 15, a particle outlet means 16, oran inner zone connecting means, etc., which are spatially connected toinner part of the fluidized bed, especially to the lower part of thefluidized bed, where the pressure is higher than that in an upper partof the inner zone 4 c, the pressure-difference controlling means maypreferably be operated so that the requirements of Po≦Pi and 0bar≦(Pi−Po)≦1 are satisfied. Then, the pressure-difference controllingmeans enables the outer zone pressure (Po) and inner zone pressure (Pi)to satisfy the requirement of 0 bar≦(Pi−Po)≦1 bar, with the innerpressure controlling means 30 being spatially connected to an inner partof the fluidized bed through a fluidizing gas inlet means 14 or areaction gas inlet means 15 or a particle outlet means 16 or an innerzone connecting means.

In contrast, it is preferred to apply and maintain a pressure-differencecontrolling means so that the requirements of Pi≦Po and 0 bar≦(Po−Pi)≦1bar may be satisfied if Pi is measured at a position that is spatiallyconnected to the upper part of the inner zone 4 c among various parts ofthe inner zone 4. Then, the pressure-difference controlling meansenables the requirement of 0 bar≦(Po−Pi)≦1 bar to be satisfied, with theinner pressure controlling means 30 being spatially connected to theinner zone 4 through a gas outlet means 17, a silicon seed crystalsinlet means 18, or an inner zone connecting means 24, 25, which are notin direct contact with the fluidized bed of silicon particles.

In the present invention, being comprised in only one of the innerpressure controlling means 30 or the outer pressure controlling means31, in both of the two controlling means 30, 31 independently, or in thetwo controlling means 30, 31 in common, the pressure-differencecontrolling means maintains the value of |Po−Pi| within 1 bar.

When the difference between Po and Pi is maintained within 1 bar byusing the pressure difference controlling means, very high or low valuesof Pi or Po do not influence on the reactor tube 2 because the pressuredifference is small between the inner zone and the outer zone of thereactor tube 2.

It is preferred in terms of productivity to maintain the reactionpressure higher than at least 1 bar instead at a vacuum state less than1 bar, if pressure is expressed in absolute unit in the presentinvention.

The feeding rates of fluidizing gas 10 and reaction gas 11 increase withpressure in a nearly proportional manner, based on mole number or massper unit time. Thus, the heat duty in the fluidized bed 4 a for heatingthe reaction gas from an inlet temperature to the temperature requiredfor reaction also increases with the reaction pressure, i.e., Po or Pi.

In case of the reaction gas 11, it is impossible to supply the gas intothe reactor after preheating up to higher than about 350-400° C., i.e.incipient decomposition temperature. Meanwhile, it is inevitable topreheat the fluidizing gas 10 up to lower than the reaction temperaturebecause impurity contamination is highly probable during a preheatingstep outside the fluidized bed reactor, and the fluidizing gas inletmeans 14 can hardly be insulated to achieve a gas preheating to abovethe reaction temperature. Therefore, difficulties in heating increasewith pressure. When the reaction pressure exceeds about 15 bar, it isdifficult to heat the fluidized bed 4 a as required although a pluralityof heating means 8 a, 8 b are additionally installed at the inner spaceof the reactor shell. Considering these practical limitations, thepressure in the outer zone 5 (Po) or the pressure in the inner zone 4(Pi) is preferred to be within about 1-15 bar based on the absolutepressure.

According to the pressure within the reactor, the inner pressurecontrolling means 30 and/or the outer pressure controlling means 31 maycomprise a pressure-difference controlling means that can reduce thepressure difference between inside and outside the reactor tube 2. Thiscan be practised in various ways, some examples of which are describedhereinafter.

The reaction pressure may be set to a high level by using thepressure-difference controlling means without deteriorating thestability of the reactor tube 2, thus enabling to increase both theproductivity and stability of the fluidized bed reactor.

For example, irrespective of the position of installation of the innerpressure controlling means 30 for ultimate connection to the inner zone4, both of the inner pressure controlling means 30 and the outerpressure controlling means 31 may comprise respectivepressure-difference controlling means so that the inner pressure (Pi) atthe inner zone 4 and the outer pressure (Po) at the outer zone 5 may becontrolled at predetermined values of pressure, i.e. Pi* and Po*,respectively, satisfying the requirement of |Po*−Pi*|≦1 bar.

For this purpose, the inner pressure controlling means 30 may comprise apressure-difference controlling means that maintains Pi at apredetermined value, Pi*. At the same time, the outer pressurecontrolling means 31 may also comprise a pressure-difference controllingmeans that maintains Po at such a predetermined value, Po*, that therequirement of |Po*−Pi*|≦1 bar is satisfied independently of the height.Likewise, the outer pressure controlling means 31 may comprise apressure-difference controlling means that maintains Po at apredetermined value, Po*. At the same time, the inner pressurecontrolling means 30 may also comprise a pressure-difference controllingmeans that maintains Pi at such a predetermined value, Pi*, that therequirement of |Po*−Pi*|≦1 bar is satisfied independently of the height.

As an another embodiment, irrespective of the position of installationof the inner pressure controlling means 30 for ultimate connection tothe inner zone 4, the inner pressure controlling means 30 may comprise apressure-difference controlling means that maintains Pi at apredetermined value, Pi*, while the outer pressure controlling means 31may comprise a pressure-difference controlling means that controls theouter pressure, Po, in accordance with the change of the real-time innerpressure so that the requirement of |Po−Pi|≦1 bar is satisfiedindependently of the height.

Meanwhile, when determining the values of the control parameters, Pi*and Po*, which are predetermined for maintaining the difference betweenPo and Po within 1 bar, it may be necessary to consider whether or notimpurity components can possibly migrate through a sealing means 41 a,41 b of reactor tube 2.

In assemblying the fluidized bed ractor for operation according to thepresent invention, there exists a practical limit that a sufficientdegree of gas-tight sealing may not be obtainable at sealing means 41 a,41 b for reactor tube 2. Further, its degree of sealing can be reducedby the shear stress imposed on reactor tube 2 due to fluidization ofsilicon particles 3. In the present invention, the problem of possiblemigration of impurity components between the inner zone 4 and the outerzone 5 through the sealing means 41 a, 41 b may be solved by properlypresetting the values of control parameters, i.e., Pi* and Po*, for thepressure-difference controlling means.

According to the present invention, the pressure control parameters tobe used at the pressure-difference controlling means for controllingpressures in the inner zone and the outer zone, respectively, may bepredetermined based on the analysis on the composition of off-gas 13 orthe gas present in outer zone 5. For example, the pattern of impuritymigration between inner zone 4 and outer zone 5 through the sealingmeans 41 a, 41 b may be deduced based on the component analysis onoff-gas 13 sampled through the gas outlet means 17 or off-gas treatingmeans 34, or that on the gas present in outer zone 5 sampled through anouter zone connecting means 28 or an inert gas connecting means 26 b. Ifoff-gas 13 is verified to comprise the constituent of inert gas 12,which is not supplied into the inner zone, the influx of impurityelements from outer zone 5 into inner zone 4 may be decreased orprevented by presetting the value of Pi* higher than that of Po*, i.e.,Pi*>Po*. In contrast, if the gas discharged out of outer zone 5 isverified to comprise the constituent of off-gas 13 of inner zone 4besides that of inert gas 12, the influx of the impurity elements frominner zone 4 into outer zone 5 may be decreased or prevented bypresetting the value of Po* higher than that of Pi*, i.e., Po*>Pi*.

As mentioned above, although the sealing means 41 a, 41 b of reactortube 2 may not be installed or maintained in a satisfactory mannerduring the assembly or operation of the fluidized bed reactor, anundesirable migration of impurity components between the two zonesthrough the sealing means may be minimized or prevented by appropriateselection of the control parameters for the pressure controlling means.Here, at whatever values Pi* and Po* may be preset in thepressure-difference controlling means, the requirement of |Po*−Pi*|≦1bar should be satisfied according to the present invention.

As another example to accomplish the object of the present invention,the pressure difference, i.e., ΔP=|Po−Pi| may be measured byinterconnecting the inner pressure controlling means 30 and the outerpressure controlling means 31, whereby the pressure-differencecontrolling means may maintain the value of ΔP within the range of 0 to1 bar, irrespective of the position of inner zone 4 selected formeasurement of Pi, by controlling the inner pressure controlling means30 and/or the outer pressure controlling means 31 in a manual,semi-automatic or automatic way.

As still another example to accomplish the object of the presentinvention, the pressure-difference controlling means may comprise anequalizing line, which spatially interconnects a connecting pipecomprised in the inner pressure controlling means 30 and a connectingpipe comprised in the outer pressure controlling means 31. A connectingpipe, which is comprised in the inner pressure controlling means 30 andconstitutes the equalizing line 23, may be installed at a positionselected for spatial connection with inner zone 4, including but notlimited to an inner zone connecting means 24, 25; a fluidizing gas inletmeans 14, 14′; a reaction gas inlet means 15; a particle outlet means16; a gas outlet means 17; or a seed crystals inlet means 18, all ofwhich are spatially exposed to the inner zone in a direct or indirectmanner. Meanwhile, a connecting pipe, which is comprised in the outerpressure controlling means 31 and constitutes an equalizing line 23, maybe installed at a position selected for spatial connection with outerzone 5, including but not limited to an outer zone connecting means 28or an inert gas connecting means 26 a, 26 b, all of which are coupledwith the reactor shell and spatially exposed to the outer zone in adirect or indirect manner.

The equalizing line 23, which interconnects spatially the inner pressurecontrolling means 30 and outer pressure controlling means 31, may bereferred to as a simplest form of the pressure-difference controllingmeans because it may always maintain the pressure difference between twointerconnected zones 4, 5 at nearly zero.

Despite this advantage, when constituting the pressure-differencecontrolling means by the equalizing line 23 alone, gas and impuritycomponents may undesirably be interchanged between two zones 4, 5. Inthis case, the impurity elements generated or discharged from aninsulating material or a heating means installed in outer zone 5 maycontaminate the inner zone 4, especially the polycrystalline siliconparticles. Likewise, silicon fine powders or components of residualreaction gas or reaction byproduct discharged from the inner zone 4 maycontaminate the outer zone 5.

Therefore, when the equalizing line 23 is used as thepressure-difference controlling means, a pressure equalizing means,which can decrease or prevent the possible interexchange of gas andimpurity components between two zones 4, 5, may be further added to theequalizing line 23. The pressure equalizing means may comprise at leastone means selected from a check valve, a pressure equalizing valve, a3-way valve, a filter for separating particles, a damping container, apacked bed, a piston, an assistant control fluid, and a pressurecompensation device using separation membrane, which, respectively, isable to prevent the possible interexchange of gas and impuritycomponents without deteriorating the effect of pressure equalization.

Besides, the pressure-difference controlling means may comprise a manualvalve for controlling pressure or flow rate, or may further comprisea(n) (semi-)automatic valve that performs a(n) (semi-)automatic controlfunction according to a predetermined value of pressure or pressuredifference. These valves may be installed in combination with a pressuregauge or a pressure indicator that exhibits a pressure or pressuredifference.

The pressure gauge or the pressure indicator is available commerciallyin the form of either analogue, digital or hybrid device, and may beincluded in an integrated system of data acquisition, storage andcontrol, if combined with a data processing means such as a signalconverter or a signal processor, etc., and/or with a local controller, adistributed controller or a central controller including a circuit forperforming an arithmetic operation.

Illustrative embodiments according to the Drawings herein are explainedhereinafter in terms of the application of the pressure-differencecontrolling means for decreasing the pressure difference between insideand outside the reactor tube 2 in the high-pressure fluidized bedreactor for preparing granular polycrystalline silicon.

BRIEF DESCRIPTION OF DRAWINGS

FIG. 1 is a cross-sectional view of a high-pressure fluidized bedreactor for preparing granular polycrystalline silicon, in which severalembodiments of the present invention are illustrated in a comprehensiveway.

FIG. 2 is a cross-sectional view of a high-pressure fluidized bedreactor for preparing granular polycrystalline silicon, in which someother embodiments according to the present invention are illustrated ina comprehensive way.

CODE EXPLANATION OF THE DRAWINGS

 1: Reactor shell  2: Reactor tube  3: silicon particles 3a: Siliconseed crystals 3b: Silicon product particles  4: Inner zone  5: Outerzone  6: Insulating material  7: Liner  8: Heater  9: Electric energy10: Fluidizing gas supplying means 11: Reaction gas 12: Inert gas 13:Off-gas 14: Fluidizing gas inlet means 15: Reaction gas inlet means 16:Particle outlet means 17: Gas outlet means 18: Silicon seed crystalsinlet means 19: Gas distributing means 23: Equalizing line 24, 25: Innerzone connecting 26: Inert gas connecting means means 27: On/off valve28: Outer zone connecting means 30: Inner pressure 31: Outer pressurecontrolling means controlling means 32: Pressure-difference gauge 33:Fluctuation reducing means 34: Off-gas treating means 35: Gas analyzingmeans 36: Filter 41: Sealing means  E: Electric source

BEST MODE FOR CARRYING OUT THE INVENTION

The present invention is described more specifically by the followingExamples. Examples herein are meant only to illustrate the presentinvention, but in no way to limit the scope of the claimed invention.

EXAMPLE 1

Hereunder is provided a description of one embodiment where the innerpressure (Pi) and the outer pressure (Po) are independently controlledat predetermined values, Pi* and Po*, respectively, and the differencebetween the values of the inner pressure and the outer pressure isthereby maintained within the range of 0 to 1 bar.

As illustrated in FIGS. 1 and 2, an inner pressure controlling means 30may be constituted by interconnecting a first pressure control valve 30b with a gas outlet means 17 through an off-gas treating means 34 forremoving fine silicon particles, which are interconnected with eachother by a connecting pipe. The pressure of the upper part of the innerzone 4 may be controlled at a predetermined value, Pi*, by using thefirst pressure control valve 30 b which behaves as an element of apressure-difference controlling means.

Meanwhile, as illustrated in FIG. 1, an outer pressure controlling means31 may be constituted by interconnecting an inert gas connecting means26 a, a fourth pressure gauge 31 a′ and a fourth pressure control valve31 b′. Although being separately installed in FIG. 1, the fourthpressure gauge 31 a′ and the fourth pressure control valve 31 b′ may beintegrated with each other by a circuit, and thus be constituted as asingle device that can measure and control pressure at the same time.

When the inner pressure controlling means 30 is connected to an upperpart of the inner zone 4 c, the pressure of which is lower than those inor below the fluidized bed, it is preferred to preset Pi* and Po* sothat the condition of Po*≧Pi* may be satisfied.

In this Example, the pressure in the outer zone may be controlled at apredetermined value, Po*, so that the condition of 0 bar≦(Po*−Pi*)≦1 barmay be satisfied, by using the fourth pressure gauge 31 a′ and thefourth pressure valve 31 b′ both of which behave as elements of apressure-difference controlling means.

However, when an inert gas 12 component is detected in the off-gas 13 bya gas analyzing means 35, which may be installed as illustrated in FIG.2, Po* may be preset at a lower value so that the condition of Pi*≧Po*may be satisfied.

Meanwhile, the inner pressure controlling means 30 and the outerpressure controlling means 31 may further comprise their ownpressure-difference controlling means, respectively, thus enabling thecondition of 0 bar≦|Po−Pi|≦1 bar to be satisfied, where Po and Pi arevalues of pressure measured in connection with the outer zone 5 and anyposition in the inner zone 4, respectively.

EXAMPLE 2

Hereunder is provided a description of another embodiment where theinner pressure (Pi) and the outer pressure (Po) are independentlycontrolled at the predetermined values, Pi* and Po*, respectively, andthe difference between the values of the inner pressure and the outerpressure is thereby maintained within the range of 0 to 1 bar.

As illustrated in FIGS. 1 and 2, an inner pressure controlling means 30may be constituted by interconnecting a first pressure control valve 30b with the gas outlet means 17 through the off-gas treating means 34 forremoving fine silicon particles, which are interconnected with eachother by a connecting pipe. The pressure of the upper part of the innerzone 4 may be controlled at a predetermined value, Pi*, by using thefirst pressure control valve 30 b which behaves as an element of apressure-difference controlling means.

Meanwhile, as illustrated in FIG. 1, an outer pressure controlling means31 may be constituted by interconnecting an inert gas connecting means26 b, an on/off valve 31 c, a third pressure gauge 31 a and a thirdpressure control valve 31 b. Although being separately installed in FIG.1, the third pressure gauge 31 a and the third pressure control valve 31b may be integrated with each other by a circuit, and thus beconstituted as a single device that can measure and control pressure atthe same time.

Unlike in Example 1, the supply of an inert gas 12 may be controlled bythe third pressure control valve 31 b in combination with the Pocontrol, instead of connecting the inert gas connecting means 26 a to apressure-difference controlling means such as the fourth pressure gauge31 a′ and the fourth pressure valve 31 b′ When the inner pressurecontrolling means 30 is connected to an upper part of the inner zone 4c, the pressure of which is lower than those in or below the fluidizedbed, it is preferred to preset Pi* and Po* so that the condition ofPo*≧Pi* may be satisfied.

In this Example, the pressure in the outer zone may be controlled at apredetermined value, Po*, so that the condition of 0 bar≦(Po*−Pi*)≦1 barmay be satisfied, by the third pressure gauge 31 a and the thirdpressure control valve 31 b both of which behave as elements of apressure-difference controlling means.

However, when an inert gas 12 component is detected in the off-gas 13 bya gas analyzing means 35, which may be installed as illustrated in FIG.2, Po* may be preset at a lower value so that the condition of Pi*≧Po*may be satisfied.

Meanwhile, the inner pressure controlling means 30 and the outerpressure controlling means 31 may further comprise their ownpressure-difference controlling means, respectively, thus enabling thecondition of 0 bar≦|Po−Pi|≦1 bar to be satisfied, where Po and Pi arevalues of pressure measured in connection with the outer zone 5 and anyposition in the inner zone 4, respectively.

EXAMPLE 3

Hereunder is provided a description of one embodiment where the innerpressure (Pi) is controlled according to the change of the outerpressure (Po), and the difference between the values of the innerpressure and the outer pressure is thereby maintained within the rangeof 0 to 1 bar.

As illustrated in FIGS. 1 and 2, a gas outlet means 17, an off-gastreating means 34 for removing fine silicon particles and a firstpressure control valve 30 b are interconnected with each other by aconnecting pipe. Then an inner pressure controlling means 30 may beconstituted by interconnecting the connecting pipe with an on/off valve27 e and a pressure-difference gauge 32.

Meanwhile, as illustrated in FIG. 1, an outer pressure controlling means31 may be constituted by interconnecting an inert gas connecting means26 b and a pressure-difference gauge 32, which are interconnected witheach other by the connecting pipe. Here an inert gas 12 may be suppliedto the outer zone through an inert gas connection means 26 a.

In the present example, the pressure-difference gauge 32 is be a commonelement for both the inner pressure controlling means 30 and the outerpressure controlling means 31. Besides the pressure control valve 31 b,31 b′ may be omitted.

When the inner pressure controlling means 30 and the outer pressurecontrolling means 31 are constituted as described above, the differencebetween the outer pressure (Po) and the inner pressure (Pi) in upperpart of the inner zone can be maintained to be lower than 1 barindependently of the change of the outer pressure (Po) by using thepressure-difference gauge 32 and the first pressure control valve 30 bboth of which behave as elements of a pressure-difference controllingmeans.

Further, the inner pressure controlling means 30 may be connected to anupper part of the inner zone 4 c, the pressure of which is lower thanthose in or below the fluidized bed, and it is preferred to control thefirst pressure control valve 30 b so that the condition of Po≧Pi may besatisfied.

However, when an inert gas 12 component may be detected in the off-gas13 by a gas analyzing means 35, which may be installed as illustrated inFIG. 2, the first pressure control valve 30 b may be controlled so thatthe condition of Pi≧Po may be satisfied.

Following the aforementioned constitution and operation of the fluidizedbed reactor, the condition of 0 bar≦|Po−Pi|≦1 bar may be satisfied atany position in the inner zone 4.

Meanwhile, the object of the present Example may be accomplished eitherby automatic control of the integrated circuit of thepressure-difference gauge 32 and the first pressure control valve 30 b,or by manual operation of the first pressure control valve 30 b inaccordance with the values of ΔP measured with the pressure-differencegauge 32.

Instead of the pressure-difference gauge 32, only a first pressure gauge30 a and a third pressure gauge 31 a may be installed as the innerpressure controlling means 30 and the outer pressure controlling means31, respectively. Alternatively, the pressure-difference controllingmeans may be further corrected or improved by equipping a first pressuregauge 30 a and a third pressure gauge 31 a in the inner pressurecontrolling means 30 and the outer pressure controlling means 31,respectively, in addition to the pressure-difference gauge 32.

EXAMPLE 4

Hereunder is provided a description of another embodiment where theinner pressure (Pi) is controlled according to the change of the outerpressure (Po), and the difference between the values of the innerpressure and the outer pressure is thereby maintained within the rangeof 0 to 1 bar.

As illustrated in FIGS. 1 and 2, an inner pressure controlling means 30may be constituted by interconnecting a first pressure control valve 30b with the gas outlet means 17 through the off-gas treating means 34 forremoving fine silicon particles, which are interconnected with eachother by a connecting pipe.

Meanwhile, as illustrated in FIG. 1, an outer pressure controlling means31 may be constituted by interconnecting an inert gas connecting means26 a for supplying an inert gas 12 and a fourth pressure gauge 31 a′,which are interconnected with each other by the connecting pipe. Here,an inert gas 12 may be discharged through an inert gas connection means26 b. Besides the pressure control valve 31 b, 31 b′ in FIG. 1 may beomitted.

When the inner pressure controlling means 30 and the outer pressurecontrolling means 31 are constituted as described above, the differencebetween the outer pressure (Po) and the inner pressure (Pi) in the upperpart of the inner zone 4 c can be maintained to be lower than 1 barindependently of the change of the outer pressure (Po) by using thefourth pressure gauge 31 a′ and the first pressure control valve 30 bboth of which behave as elements of a pressure-difference controllingmeans.

Further, since the inner pressure controlling means 30 may be connectedto an upper part of the inner zone 4 c, the pressure of which is lowerthan those in or below the fluidized bed, it is preferred to control thefirst pressure control valve 30 b so that the condition of Po≧Pi may besatisfied.

However, when an inert gas 12 component is detected in an off-gas 13 bya gas analyzing means 35, which may be installed as illustrated in FIG.2, the first pressure control valve 30 b may be controlled so that thecondition of Pi≧Po may be satisfied.

Following the aforementioned constitution and operation of the fluidizedbed reactor, the condition of 0 bar≦|Po−Pi|≦1 bar may be satisfied atany position in the inner zone 4.

Meanwhile, the object of the present Example may be accomplished eitherby automatic control of the integrated circuit of the fourth pressuregauge 31 a′ and the first pressure control valve 30 b, or by manualoperation of the first pressure control valve 30 b in accordance withthe pressure value measured with the fourth pressure gauge 31 a′.

Instead of connecting a fourth pressure gauge 31 a′ to the inert gasconnecting means 26, the outer pressure controlling means 31 may also beconstituted by connecting a fifth pressure gauge 31 p to an outer zoneconnecting means 28 as illustrated in FIG. 1 or a fifth pressure gauge31 p connected to the outer zone connecting means 28 a as illustrated inFIG. 2 or a third pressure gauge 31 a connected to an inert gasconnecting means 26 b as illustrated in FIG. 2. Then, the respectivepressure gauge employed in the outer pressure controlling means 31 mayalso behave as another element of the pressure-difference controllingmeans. Accordingly, the object of the present Example may beaccomplished by regulating the first pressure control valve 30 b, whichbehaves as an element of the pressure-difference controlling means thatis comprised in the inner pressure controlling means 30, in accordancewith the other element of the pressure-difference controlling means thatis comprised in a variety of outer pressure controlling means 31.

EXAMPLE 5

Hereunder is provided a description of one embodiment where the outerpressure (Po) is controlled according to the change of the innerpressure (Pi), and the difference between the values of the innerpressure and the outer pressure is thereby maintained within the rangeof 0 to 1 bar.

As illustrated in FIGS. 1 and 2, an inner pressure controlling means 30may be constituted by interconnecting an on/off valve 27 d and apressure-difference gauge 32 with an outer zone connecting means 25instead of the gas outlet means 17, which are interconnected with eachother by a connecting pipe.

Meanwhile, as illustrated in FIG. 1, the outer pressure controllingmeans 31 may be constituted by interconnecting a third pressure controlvalve 31 b and pressure-difference gauge 32 with an inert gas connectingmeans 26 b, which are interconnected with each other by the connectingpipe. This case corresponds to the case of constitution where the on/offvalves 27 c, 27 e are closed. In the present example, thepressure-difference gauge 32 is a common element for both the innerpressure controlling means 30 and the outer pressure controlling means31.

When the inner pressure controlling means 30 and the outer pressurecontrolling means 31 are constituted as described above, the differencebetween the outer pressure (Po) and the inner pressure (Pi) in the upperpart of the inner zone 4 c can be maintained to be lower than 1 barindependently of the change of the inner pressure (Pi) by using thepressure-difference gauge 32 and the third pressure control valve 31 bboth of which behave as elements of a pressure-difference controllingmeans.

Further, since the inner pressure controlling means 30 may be connectedto an upper part of the inner zone 4 c the pressure of which is lowerthan those in or below the fluidized bed, the third pressure controlvalve 31 b may be controlled so that the condition of Po≧Pi may besatisfied.

However, when an inert gas 12 component is detected in an off-gas 13 bya gas analyzing means 35 which may be installed as illustrated in FIG.2, the first pressure control valve 30 b may be controlled so that thecondition of Pi≧Po may be satisfied.

Following the aforementioned constitution and operation of the fluidizedbed reactor, the condition of 0 bar≦|Po−Pi|≦1 bar may be satisfied atany position in the inner zone 4.

Meanwhile, the object of the present Example may be accomplished eitherby automatic control of the integrated circuit of thepressure-difference gauge 32 and the third pressure control valve 31 b,or by manual operation of the third pressure control valve 31 b inaccordance with the ΔP value measured with the pressure-difference gauge32.

Instead of the pressure-difference gauge 32, only a first pressure gauge30 a and a third pressure gauge 31 a may be installed as the innerpressure controlling means 30 and the outer pressure controlling means31, respectively. Alternatively, the pressure-difference controllingmeans may be further corrected or improved by equipping a first pressuregauge 30 a and a third pressure gauge 31 a in the inner pressurecontrolling means 30 and the outer pressure controlling means 31,respectively, in addition to the pressure-difference gauge 32.

The outer pressure controlling means in this Example may be constitutedin another form. For example, instead of interconnection of the pressurecontrol valve 31 b and pressure-difference gauge 32 with the inert gasconnecting means 26 b in FIG. 1, the outer pressure controlling meansmay also be constituted by interconnecting the fourth pressure valve 31b′ and the pressure-difference gauge 32 with the inert gas connectingmeans 26 a for supplying the inert gas, which are interconnected witheach other by a connecting pipe. If corresponding elements of thepressure-difference controlling means is further replaced together withsuch modification of the outer pressure controlling means, the object ofthe present Example may also be accomplished thereby.

EXAMPLE 6

Hereunder is provided a description of another embodiment where theouter pressure (Po) is controlled according to the change of the innerpressure (Pi), and the difference between the values of the innerpressure and the outer pressure is thereby maintained within the rangeof 0 to 1 bar.

As illustrated in FIG. 2, the inner pressure controlling means 30 may beconstituted by interconnecting a second pressure gauge 30 a′ and apressure-difference gauge 32 with a fluidizing gas inlet means 14, whichare interconnected with each other by a connecting pipe and/or byelectrical integration.

Meanwhile, as illustrated in FIG. 2, the outer pressure controllingmeans 31 may be constituted by interconnecting a third pressure gauge 31a and a pressure-difference gauge 32, both of which are connected to aninert gas connecting means 26 b, with a second pressure control valve 30b′ which is connected to an inert gas connecting means 26 a. Here, theinterconnection may be achieved by the connecting pipe and/or byelectrical integration.

In the present example, the pressure-difference gauge 32 is a commonelement for both the inner pressure controlling means 30 and the outerpressure controlling means 31. The pressure-difference gauge 32 exhibitsa physical and/or electrical signal for the difference between Pi andPo, which are measured with the second pressure gauge 30 a′ and thethird pressure gauge 31 a, respectively.

A fluctuation reducing means 33 may further be applied to thepressure-difference gauge because the fluidization of silicon particlesin the fluidized bed naturally introduces fluctuation in the value of Pimeasured by the second pressure gauge 30 a′. The fluctuation reducingmeans 33 may comprise a pressure fluctuation damping (or buffering)means such as a physical device or a software-based device thattransforms the fluctuating signals into an average Pi value for apredetermined short period of time (e.g., one second).

Then, by using the pressure-difference gauge 32 and the second pressurecontrol valve 30 b′ both of which behave as elements of apressure-difference controlling means, the difference between the outerpressure (Po) and the inner pressure (Pi) is maintained to be lower than1 bar independently of the change of the inner pressure (Pi) measuredthrough the fluidizing gas inlet means 14 in connection with the innerzone.

Further, since the inner pressure controlling means 30 may be connectedto a lower part of the fluidized bed, the pressure of which is higherthan that in upper part of the inner zone 4 c, the second pressurecontrol valve 30 b′ may be controlled so that the condition of Po≦Pi maybe satisfied.

However, when an off-gas 13 component is detected in an inert gas 12′ bya gas analyzing means 35, which may be installed as illustrated in FIG.2, the second pressure control valve 30 b′ may be controlled so that thecondition of Po≧Pi may be satisfied.

Following the aforementioned constitution and operation of the fluidizedbed reactor, the condition of 0 bar≦|Po−Pi|≦1 bar may be satisfied atany position in the inner zone 4.

Meanwhile, the object of the present Example may be accomplished eitherby automatic control of the integrated circuit of thepressure-difference gauge 32 and the second pressure control valve 30b′, or by manual operation of the second pressure control valve 30 b′ inaccordance with the ΔP value measured with the pressure-difference gauge32.

Further, on behalf of the third pressure gauge 31 a in connection withthe inert gas connecting means 26 b, another outer pressure gauge may beconnected to the pressure-difference gauge 32 for achieving the objectof the present Example. For example, the outer pressure gauge may alsobe selected from the fifth pressure gauge 31 p in connection with theouter zone connecting means 28 a or a sixth pressure gauge 31 q inconnection with the inert gas connecting means 26 a.

EXAMPLE 7

Hereunder is provided a description of one embodiment where thedifference between the values of the inner pressure and the outerpressure is maintained within the range of 0 to 1 bar by using anequalizing line spatially interconnecting the inner zone and the outerzone.

As illustrated in FIG. 1, the equalizing line 23 may be composed of aconnecting pipe which spatially interconnects an inner zone connectingmeans 25 with an inert gas connecting means 26 b.

In this case, the inner pressure controlling means 30 may be basicallycomposed of the inner zone connecting means 25 and the connecting pipe,and may further comprise an on/off valve 27 d and a first pressure gauge30 a as illustrated in FIG. 1. Meanwhile, the outer pressure controllingmeans 31 may be basically composed of a connecting means, which isselected among an inert gas connecting means 26 a or an outer zoneconnecting means 28, and the connecting pipe, and may further comprisean on/off valve 31 c and a third pressure gauge 31 a as illustrated inFIG. 1.

In the present Example, an equalizing line 23 is composed of the twoconnecting pipes that constitute the inner pressure controlling means 30and the outer pressure controlling means 31, respectively. Therefore,the equalizing line 23 behaves, by itself, as a pressure-differencecontrolling means. Spatially interconnecting the upper part of the innerzone 4 c with the outer zone 5, the equalizing line 23 naturallyprevents an apparent pressure difference between these two zones.

The pressure difference between Pi, measured at a lower part of thefluidized bed 4 a where Pi is highest in the bed, and Po, measured at anupper part of the inner zone 4 c, is usually below 1 bar. Thus, if theequalizing line 23 is used as the pressure-difference controlling means,the pressure difference between Pi and Po, i.e., between inside andoutside of the reactor tube 2 may be maintained below 1 bar irrespectiveof the measurement point of Pi.

The object of the present Example may also be accomplished by selectinga space in connection with a gas outlet means 17, instead of the innerzone connecting means 25, for constituting the inner pressurecontrolling means 30.

Meanwhile, the effect of pressure equalization of Pi and Po attributedto the equalizing line 23, which is a pressure-difference controllingmeans in the present Example, may also be obtained when a pressureequalizing valve 27 c is further equipped at the equalizing line 23enabling spatial partition of the inner zone and the outer zone.

EXAMPLE 8

Hereunder is provided a description of another embodiment where thedifference between the values of the inner pressure and the outerpressure is maintained within the range of 0 to 1 bar by using anequalizing line spatially interconnecting the inner zone and the outerzone

As illustrated in FIG. 2, the equalizing line 23 may be composed of aconnecting pipe which spatially interconnects an inner zone connectingmeans 25 and an outer zone connecting means 28 b. In this case, theinner pressure controlling means 30 may be basically composed of theinner zone connecting means 25 and the connecting pipe. Meanwhile, theouter pressure controlling means 31 may be basically composed of theouter zone connecting means 28 b and the connecting pipe.

In the present Example, an equalizing line 23 is composed of the twoconnecting pipes that constitute the inner pressure controlling means 30and the outer pressure controlling means 31, respectively. Therefore,the equalizing line 23 behaves, by itself, as a pressure-differencecontrolling means. Spatially interconnecting the upper part of the innerzone 4 c with the outer zone 5, the equalizing line 23 naturallyprevents an apparent pressure difference between these two zones.

The pressure difference between Pi, measured at a lower part of thefluidized bed 4 a where Pi is highest in the bed, and Po, measured at anupper part of the inner zone 4 c, is usually below 1 bar. Thus, if theequalizing line 23 is used as the pressure-difference controlling means,the pressure difference between Pi and Po, i.e., between inside andoutside of the reactor tube 2 may be maintained below 1 bar irrespectiveof the measurement point of Pi.

Meanwhile, to prevent the migration of impure particles and componentsthrough the equalizing line 23, a filter 36 and/or an on/off valve 27 dmay be further equipped at the equalizing line 23 as illustrated in FIG.2.

EXAMPLE 9

Hereunder is provided a description of still another embodiment wherethe difference between the values of the inner pressure and the outerpressure is maintained within the range of 0 to 1 bar by using anequalizing line spatially interconnecting the inner zone and the outerzone.

As illustrated in FIG. 2, the equalizing line 23 may be composed of aconnecting pipe which spatially interconnects a gas outlet means 17 withan inert gas connecting means 26 b.

In this case, the inner pressure controlling means 30 may be basicallycomposed of the gas outlet means 17, an off-gas treating means 34 andthe connecting pipe, and may further comprise a first pressure gauge 30a, an on/off valve 31 d, a filter 36, etc., as illustrated in FIG. 2.Meanwhile, the outer pressure controlling means 31 may be basicallycomposed of a connecting means, which is selected among an inert gasconnecting means 26 a or an outer zone connecting means 28, and theconnecting pipe, and may further comprise an on/off valves 31 b, 31 e,31 f, 31 g, a gas analyzing means 35 and a third pressure gauge 31 a,etc., as illustrated in FIG. 2.

In the present Example, an equalizing line 23 is composed of the twoconnecting pipes that constitute the inner pressure controlling means 30and the outer pressure controlling means 31, respectively. Therefore,the equalizing line 23 behaves, by itself, as a pressure-differencecontrolling means. Spatially interconnecting the upper part of the innerzone 4 c with the outer zone 5; the equalizing line 23 naturallyprevents an apparent pressure difference between these two zones.

The pressure difference between Pi, measured at a lower part of thefluidized bed 4 a where Pi is highest in the bed, and Po, measured at anupper part of the inner zone 4 c, is usually below 1 bar. Thus, if theequalizing line 23 is used as the pressure-difference controlling means,the pressure difference between Pi and Po, i.e., between inside andoutside of the reactor tube 2 may be maintained below 1 bar irrespectiveof the measurement point of Pi.

The object of the present Example may also be accomplished when areaction gas inlet means 15 is interconnected with the outer zone 5 byselecting a space in connection with a reaction gas inlet means 15,instead of the gas outlet means 17, for constituting the inner pressurecontrolling means 30.

Meanwhile, the effect of pressure equalization of Pi and Po attributedto the equalizing line 23, which is a pressure-difference controllingmeans in the present Example, may also be obtained when a pressureequalizing valve 27 c in FIG. 2 is further equipped at the equalizingline 23 enabling spatial partition of the inner zone and the outer zone.

EXAMPLE 10

Hereunder is provided a description of still another embodiment wherethe outer pressure (Po) is controlled according to the change of theinner pressure (Pi), and the difference between the values of the innerpressure and the outer pressure is thereby maintained within the rangeof 0 to 1 bar.

In the present Example, an average value of the inner pressure, Pi(avg),may be estimated from the two values of pressure measured at two spaceswhich are in spatial connection with a fluidizing gas inlet means 14 anda gas outlet means 17 independently. Then, Po may be controlledaccording to the estimated value of Pi(avg), thus maintaining thedifference between the values of Pi and Po within 1 bar, preferably 0.5bar.

In the present Example, a second pressure gauge 30 a′ and a firstpressure gauge 30 a are installed in connection with a fluidizing gasinlet means 14 and a gas outlet means 17, respectively. The innerpressure controlling means 30 may be constituted as an integratedcircuit of a pressure-difference gauge 32 of FIG. 2 and a controllercomprising an arithmetic processor, where the controller generates anestimated value of Pi(avg) based on the real-time measurements of thetwo pressure gauges 30 a′, 30 a. Meanwhile, as illustrated in FIG. 2, anouter pressure controlling means 31 may be constituted as an integratedcircuit of the pressure-difference gauge 32 as well as a second pressurecontrol valve 30 b′ and a third pressure gauge 31 a which are connectedto an inert gas connecting means 26 a and an inert gas connecting means26 b, respectively. Here, the pressure-difference gauge 32 exhibits thedifference between Pi(avg) and Po, and generates an electric signalcorresponding to the difference, thus operating the second pressurecontrol valve 30 b′. Therefore, being a common element for both theinner pressure controlling means 30 and the outer pressure controllingmeans 31, the software-based function of the pressure-difference gauge32 may be coupled into the controller for estimation of Pi(avg).

Because the value of Pi measured by the second pressure gauge 30 a′fluctuates depending on the fluidization state of the fluidized bed, thecontroller comprising an arithmetic processor for estimation of Pi(avg)may further comprise a software-based damping means that generatestime-averaged values of pressure, Pi*(avg), at an interval of, forexample, 10 seconds or 1 minute based on the fluctuating real-timevalues of Pi. This damping means may allow a smooth operation of thesecond pressure control valve 30 b′ based on the time-averaged valueinstead of the fluctuating Pi.

Using the controller comprising an arithmetic processor and the secondpressure control valve 30 b′ as a pressure-difference controlling means,it is possible to control the outer pressure (Po) according to thechange of the time-average of Pi values measured at different positionsin connection with the inner zone, and then to maintain the differenceof Po from and Pi(avg) or Pi*(avg) within the range of 0 to 1 bar.

The manipulation of the second pressure control valve 30 b′ forcontrolling the outer pressure according to the average value of theinner pressure may be adjusted following a gas-component analysis on theoff-gas through a gas outlet means 17 or the off-gas treating means 34and/or on the gas discharged from the outer zone through the outer zoneconnecting means 28 or an inert gas connecting means 26 b. If a largeamount of an inert gas component is detected in the off-gas, it ispreferred to lower Po, thus decreasing the migration of impurity intothe inner zone 4 from the outer zone 5. On the contrary, if an off-gas13 component is detected in the gas from the outer zone besides an inertgas 12, it is preferred to raise Po, thus decreasing the migration ofimpurity into the outer zone 5 from the inner zone 4. Nonetheless,according to the present Example, the condition of |Po−Pi*(avg)|≦1 barshould be satisfied irrespective of conditions for controlling Po. Ifthe impurity component is not detected, it is preferred to manipulatethe second pressure control valve 30 b′ so that Po may be substantiallythe same with Pi*(avg). Therefore, it is possible to minimize or preventthe undesirable migration of impurity by controlling the pressuredifference between the inner zone 4 and the outer zone 5, although thesealing means 41 a, 41 b for reactor tube 2 are not maintained perfectduring the operation of the fluidized bed reactor.

The object of the present Example may also be accomplished byconstituting the outer pressure controlling means 31 in a different way.For example, instead of the third pressure gauge 31 a connected to theinert gas connecting means 26 b, a fifth pressure gauge 31 p or a sixthpressure gauge 31 q, which are connected to an outer zone connectingmeans 28 a or an inert gas connecting means 26 a, respectively, to maybe selected as the pressure gauge to be connected to thepressure-difference gauge 32. Further, instead of the second pressurecontrol valve 30 b′ connected to the inert gas connecting means 26 a, athird pressure control valve 31 b connected to the inert gas connectingmeans 26 b may be selected as the pressure control valve.

Meanwhile, the object of the present Example may also be accomplished byconstituting the inner pressure controlling means 30 in a different way.For example, instead of the second pressure gauge 30 a′ connected to thefluidizing gas inlet means 14, a pressure gauge in spatial connectionwith a silicon product particle outlet means 16 may be selected formeasurement of Pi(avg) together with the first pressure gauge 30 aconnected to the gas outlet means 17.

Besides the aforementioned Examples, the inner pressure controllingmeans 30, the outer pressure controlling means 31 and thepressure-difference controlling means may be constituted in a variety ofmanners for preparation of granular polycrystalline silicon according tothe present invention.

As set forth above, the high-pressure fluidized bed reactor forpreparing granular polycrystalline silicon herein have the superiorityas follows.

1. The pressure difference between both sides of the reactor tube ismaintained so low that a high-pressure silicon deposition is possiblewithout deteriorating the physical stability of the reactor tube, thusenabling to fundamentally prevent the damage of the reactor tube due tothe pressure difference, and to increase long-term stability of thereactor.

2. The silicon deposition reaction may be performed even at highpressure, thus enabling to remarkably increase the production yield ofpolycrystalline silicon per fluidized bed reactor.

3. It is possible to lower the cost for preparing the reactor tubebecause the material or thickness of the reactor tube may be determinedwithout being affected by pressure.

4. The difference between the inner and the outer pressure may bemaintained within a predetermined range at a relatively low cost withoutcontinuously providing a large amount of inert gas into the outer zoneof the reactor.

5. The outer zone of the reactor is maintained under an inert gasatmosphere and the inert gas may be discharged through a separate exit.Thus, although an insulating material and optionally a heater areinstalled in the outer zone and the outer zone may comprise additionalpartitioning means in a radial or vertical direction, it is possible todecrease remarkably the possibility that impurity from these componentscan migrate into the inner zone and deteriorate the quality ofpolycrystalline silicon product.

6. The long-term stability of the reactor may be increased remarkablybecause any thermal degradation in terms of chemical and physicalproperties of those additional components in the outer zone is lessprobable under the inert gas atmosphere.

7. Even in case the components of fluidizing gas, reaction gas oroff-gas, or fine silicon particles happen to migrate into the outer zonefrom the inner zone, they may be easily removed therefrom by the inertgas introduced into the outer zone, thus enabling to prevent aninterruption of operation due to contamination in the outer zone.

1. A high-pressure fluidized bed reactor for preparing granularpolycrystalline silicon, comprising: (a) a reactor tube; (b) a reactorshell encompassing the reactor tube; (c) an inner zone formed within thereactor tube and an outer zone formed in between the reactor shell andthe reactor tube, wherein a silicon particle bed is formed and silicondeposition occurs in the inner zone while a silicon particle bed is notformed and silicon deposition does not occur in the outer zone; (d) aninlet means for introducing gases into the silicon particle bed; (e) anoutlet means comprising a silicon particle outlet means and a gas outletmeans for discharging the polycrystalline silicon particles and off-gasout of the silicon particle bed, respectively; (f) an inert gasconnecting means for maintaining a substantially inert gas atmosphere inthe outer zone; (g) a pressure controlling means for measuring and/orcontrolling the inner zone pressure (Pi) or the outer zone pressure(Po); and (h) a pressure-difference controlling means for maintainingthe value of |Po−Pi| within the range of 0 to 1 bar.
 2. The reactor ofclaim 1, wherein the inlet means comprises a fluidizing gas inlet meansfor introducing a fluidizing gas to the silicon particle bed and areaction gas inlet means for introducing a silicon atom-containingreaction gas to the silicon particle bed.
 3. The reactor of claim 1,wherein the outlet means comprises a silicon particle outlet means fordischarging polycrystalline silicon particles formed in the inner zoneout of the fluidized bed reactor and a gas outlet means for dischargingoff-gas including a fluidizing gas, a non-reacted reaction gas and abyproduct gas.
 4. The reactor of claim 1, wherein the pressurecontrolling means comprises an inner pressure controlling means which isspatially connected to the inner zone through at least one meansselected from the group consisting of an inner zone connecting means, afluidizing gas inlet means, a reaction gas inlet means, a siliconparticle outlet means and a gas outlet means, which are spatiallyexposed to the inner zone.
 5. The reactor of claim 1, wherein thepressure controlling means comprises an outer pressure controlling meanswhich is spatially connected to the outer zone through at least onemeans selected from the group consisting of an outer zone connectingmeans and an inert gas connecting means, which are installed on orthrough the reactor shell 1 and spatially exposed directly or indirectlyto the outer zone
 5. 6. The reactor of claim 1, wherein the inert gas isat least one gas selected from the group consisting of hydrogen,nitrogen, argon and helium.
 7. The reactor of claim 1, wherein thereactor tube is made of at least one material selected from the groupconsisting of quartz, silica, silicon nitride, boron nitride, siliconcarbide, graphite, silicon, and glassy carbon.
 8. The reactor of claim7, wherein the reactor tube is of one-layered or multi-layered structurein the thickness direction, each layer of which is made of a differentmaterial.
 9. The reactor of claim 1, wherein at least one heating meansis installed in the inner zone and/or the outer zone.
 10. The reactor ofclaim 9, wherein the heating means is electrically connected to anelectric energy supplying means installed on or through the reactorshell.
 11. The reactor of claim 1, wherein the heating means isinstalled within the silicon particle bed.
 12. The reactor of claim 11,wherein the heating means is positioned lower than a reaction gas inletmeans for introducing a reaction gas to into the silicon particle bed.13. The reactor of claim 1, wherein the pressure controlling meanscomprises the pressure-difference controlling means.
 14. The reactor ofclaim 1, wherein the inner zone pressure and the outer zone pressure arein the range of 1-15 bar, respectively.
 15. The reactor of claim 14,wherein the outer zone pressure may be controlled in the range ofbetween maximum and minimum pressure values measurable in the innerzone.
 16. The reactor of claim 1, wherein the pressure controlling meansincludes at least one component selected from the group consisting of:(a) a connecting pipe or fitting for spatial connection; (b) amanually-operated, semi-automatic, or automatic valve; (c) a digital oranalog pressure gauge or pressure-difference gauge; (d) a pressureindicator or recorder; and (e) an element constituting a controller witha signal converter or an arithmetic processor.
 17. The reactor of claim1, the pressure controlling means for the inner pressure isinterconnected with the pressure controlling means for the outerpressure in the form of a mechanical assembly or a signal circuit. 18.The reactor of claim 17, wherein the pressure controlling means ispartially or completely integrated with a control system selected fromthe group consisting of a central control system, a distributed controlsystem and a local control system.
 19. The reactor of claim 17, whereinthe pressure controlling means is partially or completely integratedwith a means for measuring or controlling a parameter selected from thegroup consisting of flow rate, temperature, gas component and particleconcentration.
 20. The reactor of claim 17, wherein the pressurecontrolling means comprises a filter or a scrubber for separatingparticles, or a container for buffering pressure.
 21. The reactor ofclaim 1, wherein the pressure-difference controlling means comprises atleast one selected from the group consisting of a connecting pipe, amanually-operated valve, an automatic valve, a pressure gauge, apressure indicator, a signal converter, a controller with an arithmeticprocessor and a filter for separating particles.
 22. The reactor ofclaim 1, wherein the inner pressure controlling means and the outerpressure controlling means comprise respective pressure-differencecontrolling means so that the inner pressure (Pi) at the inner zone andthe outer pressure (Po) at the outer zone be controlled at predeterminedvalues of pressure, i.e. Pi* and Po*, respectively, satisfying therequirement of |Po*−Pi*|≦1 bar.
 23. The reactor of claim 1, wherein thepressure difference, i.e., ΔP=|Po−Pi| is measured by interconnecting theinner pressure controlling means and the outer pressure controllingmeans, whereby the pressure-difference controlling means maintains thevalue of ΔP within the range of 0 to 1 bar by controlling the innerpressure controlling means and/or the outer pressure controlling meansin a manual, semi-automatic or automatic way.
 24. The reactor of claim1, the pressure-difference controlling means comprises an equalizingline that spatially interconnects a first connecting pipe and a secondconnecting pipe, which are comprised in the inner pressure controllingmeans and the outer pressure controlling means, respectively.
 25. Thereactor of claim 24, the equalizing line comprises at least one selectedfrom the group consisting of a check valve, a pressure equalizing valve,a 3-way valve, a filter for separating particles, a damping container, apacked bed, a piston, an assistant control fluid and a pressurecompensation device using separation membrane.